Efficient Electrocatalytic Ammonia Synthesis via Theoretical Screening of Titanate Nanosheet-Supported Single-Atom Catalysts

• Published in: Materials Vol. 17; no. 10; p. 2239
• Main Authors: Zhao, Kaiheng, Wang, Jingnan, Yang, Yongan, Wang, Xi
• Format: Journal Article
• Language: English
• Published: Switzerland MDPI AG 09.05.2024
• Subjects: Ammonia; Catalysts; Chemical reduction; Chemical synthesis; Density functional theory; Efficiency; Electrodes; Electrolytes; Energy consumption; Hydrogen; Hydrogen evolution reactions; Hydrogenation; Nanosheets; NRR; Potassium; Radiation; Scanning electron microscopy; Screening; Single atom catalysts; theoretical screening; China; United States > US; single-atom catalysts; theoretical screening; NRR
• ISSN: 1996-1944; 1996-1944
• DOI: 10.3390/ma17102239

The electrocatalytic nitrogen reduction reaction (NRR) for synthesizing ammonia holds promise as an alternative to the traditional high-energy-consuming Haber-Bosch method. Rational and accurate catalyst design is needed to overcome the challenge of activating N and to suppress the competitive hydrogen evolution reaction (HER). Single-atom catalysts have garnered widespread attention due to their 100% atom utilization efficiency and unique catalytic performance. In this context, we constructed theoretical models of metal single-atom catalysts supported on titanate nanosheets (M-TiNS). Initially, density functional theory (DFT) was employed to screen 12 single-atom catalysts for NRR- and HER-related barriers, leading to the identification of the theoretically optimal NRR catalyst, Ru-TiNS. Subsequently, experimental synthesis of the Ru-TiNS single-atom catalyst was successfully achieved, exhibiting excellent performance in catalyzing NRR, with the highest NH yield rate reaching 15.19 μmol mg h and a Faradaic efficiency (FE) of 15.3%. The combination of experimental results and theoretical calculations demonstrated the efficient catalytic ability of Ru sites, validating the effectiveness of the constructed theoretical screening process and providing a theoretical foundation for the design of efficient NRR catalysts.